3'-Acetylrinderine, 3'-acetylechinatine, 3-acetylheliosupine and heliosupine were isolated from the aerial parts of Cynoglossum creticum and characterized by mass spectrometry and H-1 and C-13 NMR. A GC-mass spectrometric analysis revealed the presence of 13 alkaloids altogether, among them the previously reported alkaloids, echinatine, rinderine and 7-angeloylheliotridine, and traces of 7-senecioylheliotridine, supinine and trachelanthamine.